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Y2O3负载金属Cu在催化甲醛水溶液制氢反应中的Y2O3载体效应

Effect of Y2O3 Supporter on the Catalytic Hydrogen Production from an Aqueous Formaldehyde Solution Catalyzed by Metal Cu Loaded on Y2O3

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【作者】 田毅李越湘彭绍琴

【Author】 TIAN Yi;LI Yuexiang;PENG Shaoqin;College of Chemistry,Nanchang University;

【机构】 南昌大学化学学院

【摘要】 采用NaBH4还原法将纳米金属Cu负载在Y2O3上.通过X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)和测定氢氧根在Y2O3和Cu上的吸附等手段对样品进行了表征.结果表明,Y2O3表面存在一层薄的Y(OH)3,能优先吸附OH-使其在Y2O3表面"富集";金属Cu以纳米粒子形式负载在Y2O3上.在碱性甲醛溶液中考察了Y2O3负载Cu(Cu/Y2O3)的催化性能.结果表明,在低碱度条件下,相对于未负载纳米Cu的Y2O3,Cu/Y2O3具有较高的产氢活性.当氢氧化钠浓度为0.050 mol/L时,在氮气气氛下Cu/Y2O3产氢量约为未负载纳米Cu的7.8倍;而在空气气氛下约为4.3倍.在2种气氛下,Cu/Y2O3产氢的最佳氢氧化钠浓度均为0.25 mol/L.这可归结为Y2O3表面对OH-的"富集"效应,使其表面产生更多的活性物种CH2(OH)O-(甲二醇负离子).相对于未负载纳米Cu的Y2O3,Y2O3负载Cu提高了催化剂的稳定性,其原因是Y2O3负载阻止了Cu粒子在反应过程的生长.

【Abstract】 Nano metal Cu was loaded on Y2O3 by NaBH4 reduction method. The sample was characterized by X-ray diffraction( XRD),X-ray photoelectron spectroscopy( XPS),transmission electron microscopy( TEM)and adsorption measurement of OH-on Y2O3 and Cu. The results show that there is a thin layer of Y( OH)3on the surface of Y2O3,which can preferentially adsorb OH-,that is,"enrichment"of OH-on Y2O3; metal Cu was loaded on Y2O3 in the form of nano particles. The performance of Cu supported on Y2O3( Cu/Y2O3)catalyst was investigated in alkaline formaldehyde solution. The results show that under low alkalinity,Cu/Y2O3 exhibits higher activity for hydrogen production than unloaded nano metal Cu. When the concentration of Na OH is 0. 050 mol/L,the hydrogen amount produced over Cu/Y2O3 is 7. 8 times as high as that over nano Cu under N2 atmosphere,whereas the former is 4. 3 times as high as the latter under air atmosphere. The optimal Na OH concentration for hydrogen production over Cu/Y2O3 is 0. 25 mol/L under both atmospheres. The results can be attributed to "enrichment"effect of OH-on Y2O3,leading to production of the higher concentration of active CH2( OH) O-( formaldehyde anion) species on Y2O3. The stability of Cu/Y2O3 is improved compared with that of unloaded nano Cu. The reason is that the load of Cu on Y2O3 prevents growth of Cu particles during the reaction.

【关键词】 甲醛制氢负载铜Y2O3OH-富集
【Key words】 FormaldehydeHydrogen productionLoad of CuY2O3Enrichment of OH-
【基金】 国家自然科学基金(批准号:21563019,21366022);化工资源有效利用国家重点实验室开放课题(批准号:CRE-2016-C-102);江西省自然科学基金(批准号:20151BAB203013)资助~~
  • 【文献出处】 高等学校化学学报 ,Chemical Journal of Chinese Universities , 编辑部邮箱 ,2017年10期
  • 【分类号】O643.36;TQ116.2
  • 【被引频次】8
  • 【下载频次】214
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